By correlating time- and angle-resolved photoemission (Tr-ARPES) and time-resolved transverse- magneto-optical Kerr effect (Tr-TMOKE) measurements, both at extreme ultraviolet (EUV) wavelengths, we uncover the nature of the ultrafast photoinduced magnetic phase transition in Ni. This allows us to explain the ultrafast magnetic response of Ni at all laser fluences - from a small reduction of the magnetization at low laser fluences, to complete quenching at high laser fluences. We provide an alternative explanation to the fluence-dependent recovery timescales commonly observed in ultrafast magneto-optical spectroscopies on ferromagnets: it is due to the bulk-averaging effect and different depths of sample exhibit distinct dynamics, depending on whether a magnetic phase transition is induced. We also show evidence of two competing channels with two distinct timescales in the recovery process, that suggest the presence of coexisting phases in the material.

We use attosecond pulses to measure the fastest intrinsic processes in solids. Our results reveal the influence of the band structure on excited-state lifetimes and extract fundamental electron interactions including attosecond electron screening and scattering.

It has long been known that ferromagnets undergo a phase transition from ferromagnetic to paramagnetic at the Curie temperature, associated with critical phenomena such as a divergence in the heat capacity. A ferromagnet can also be transiently demagnetized by heating it with an ultrafast laser pulse. However, to date the connection between out-ofequilibrium and equilibrium phase transitions was not known, nor how fast the out-of-equilibrium phase transitions can proceed. In this work, by combining time- and angle-resolved photoemission (Tr-ARPES) with time-resolved transverse magneto-optical Kerr (Tr-TMOKE) spectroscopies, we show that the same critical behavior also governs the ultrafast magnetic phase transition in nickel. This is evidenced by several observations. First, we observe a divergence of the transient heat capacity of the electron spin system preceding material demagnetization. Second, when the electron temperature is transiently driven above the Curie temperature, we observe an extremely rapid change in the material response: the spin system absorbs sufficient energy within the first 20 fs to subsequently proceed through the phase transition, while demagnetization and the collapse of the exchange splitting occur on much longer timescales. Third, we find that the transient electron temperature alone dictates the magnetic response. By comparing results obtained from different methods, we show that the critical behaviors are essential for fully explaining the fluence-dependent magnetization dynamics measured using magneto-optical spectroscopy

By correlating time- and angle-resolved photoemission and time-resolved transverse magneto-optical Kerr effect measurements, both at extreme ultraviolet wavelengths, we uncover the universal nature of the ultrafast photoinduced magnetic phase transition in Ni. This allows us to explain the ultrafast magnetic response of Ni at all laser fluences-from a small reduction of the magnetization at low laser fluences, to complete quenching at high laser fluences. Both probe methods exhibit the same demagnetization and recovery timescales. The spin system absorbs the energy required to proceed through a magnetic phase transition within 20 fs after the peak of the pump pulse. However, the spectroscopic signatures of demagnetization of the material appear only after ≈200  fs and the subsequent recovery of magnetization on timescales ranging from 500 fs to >70  ps. We also provide evidence of two competing channels with two distinct timescales in the recovery process that suggest the presence of coexisting phases in the material.

It has long been known that ferromagnets undergo a phase transition from ferromagnetic to paramagnetic at the Curie temperature, associated with critical phenomena such as a divergence in the heat capacity. A ferromagnet can also be transiently demagnetized by heating it with an ultrafast laser pulse. However, to date, the connection between out-of-equilibrium and equilibrium phase transitions, or how fast the out-of-equilibrium phase transitions can proceed, was not known. By combining time- and angle-resolved photoemission with time-resolved transverse magneto-optical Kerr spectroscopies, we show that the same critical behavior also governs the ultrafast magnetic phase transition in nickel. This is evidenced by several observations. First, we observe a divergence of the transient heat capacity of the electron spin system preceding material demagnetization. Second, when the electron temperature is transiently driven above the Curie temperature, we observe an extremely rapid change in the material response: The spin system absorbs sufficient energy within the first 20 fs to subsequently proceed through the phase transition, whereas demagnetization and the collapse of the exchange splitting occur on much longer, fluence-independent time scales of ~176 fs. Third, we find that the transient electron temperature alone dictates the magnetic response. Our results are important because they connect the out-of-equilibrium material behavior to the strongly coupled equilibrium behavior and uncover a new time scale in the process of ultrafast demagnetization.

Electron-electron interactions are the fastest processes in materials, occurring on femtosecond to attosecond timescales, depending on the electronic band structure of the material and the excitation energy. Such interactions can play a dominant role in light-induced processes such as nano-enhanced plasmonics and catalysis, light harvesting, or phase transitions. However, to date it has not been possible to experimentally distinguish fundamental electron interactions such as scattering and screening. Here, we use sequences of attosecond pulses to directly measure electron-electron interactions in different bands of different materials with both simple and complex Fermi surfaces. By extracting the time delays associated with photoemission we show that the lifetime of photoelectrons from the d band of Cu are longer by ∼100 as compared with those from the same band of Ni. We attribute this to the enhanced electron-electron scattering in the unfilled d band of Ni. Using theoretical modeling, we can extract the contributions of electron-electron scattering and screening in different bands of different materials with both simple and complex Fermi surfaces. Our results also show that screening influences high-energy photoelectrons (≈20 eV) significantly less than low-energy photoelectrons. As a result, high-energy photoelectrons can serve as a direct probe of spin-dependent electron-electron scattering by neglecting screening. This can then be applied to quantifying the contribution of electron interactions and screening to low-energy excitations near the Fermi level. The information derived here provides valuable and unique information for a host of quantum materials.

Tabletop-scale coherent EUV generated through high-harmonic generation (HHG) produces light in the form of an attosecond pulse train that uniquely combines characteristics of good energy resolution (approximate to 100-300meV) with sub-fs time resolution. This makes HHG an ideal source for studying the fastest dynamics in materials. Furthermore, using angle-resolved photoemission spectroscopy (ARPES), it is possible to extract detailed information about electron dynamics over the entire Brillouin zone. In recently published work, we combined HHG with ARPES to identify a sub-femtosecond excited-state lifetime for the first time. Photoemission occurs as a three-step process: 1) An electron is photoexcited from the valence band to far above the Fermi energy; 2) it transports to the surface, and 3) it overcomes the work function and exits. If the electron is promoted into a highlyexcited unoccupied band in the material (as opposed to a free-electron-like state), we observe the electron emission lifetime to increase in a measurable way-the Ni band 22 eV above the Fermi level has a lifetime of 212 +/- 30 attoseconds. Furthermore, by comparing photoemission from Cu and Ni, we reveal the influence of attosecond-timescale electron screening vs scattering by the electrons near the fermi surface. This work for the first time demonstrates the relevance of attosecond spectroscopy to the study of intrinsic properties and band structure in materials, as opposed to the strong-field induced dynamics studied extensively to-date.

By correlating time- and angle-resolved photoemission and time-resolved transverse- magneto- optical Kerr effect measurements, both at extreme ultraviolet wavelengths, we uncover the universal nature of the ultrafast photoinduced magnetic phase transition in Ni. This allows us to explain the ultrafast magnetic response of Ni at all laser fluences - from a small reduction of the magnetization at low laser fluences, to complete quenching at high laser fluences. Both probe methods exhibit the same demagnetization and recovery timescales. We further show that the ultrafast demagnetization in Ni is indeed a magnetic phase transition that is launched within 20 fs, followed by demagnetization of the material within ~200 fs, and subsequent recovery of the magnetization on timescales ranging from 500 fs to >70 ps. We also provide evidence of two competing channels with two distinct timescales in the recovery process, that suggest the presence of coexisting phases in the material.

Attosecond pulses and pulse trains generated by high-order harmonic generation are finding broad applications in advanced spectroscopies and imaging, enabling sub-femtosecond electron dynamics to be probed in atomic, molecular and material systems. To date, isolated attosecond pulses have been generated either by using very short few-cycle driving pulses, or by using temporal and polarization gating, or by taking advantage of phase-matching gating. Here we show that by driving high harmonics with a two-color linearly polarized laser field, the temporal window for time-gated phase matching is shorter than for the equivalent singe-color driving laser. As a result, we can generate quasi-isolated attosecond pulses with a peak width of similar to 450 as using relatively long 26 femtosecond laser pulses. Our experimental data are in good agreement with theoretical simulations, and show that the phase matching window decreases by a factor of 4 - from four optical cycles in the case of a single-color fundamental driving laser, to one optical cycle in the case of two-color (omega-2 omega) laser drivers. Finally, we also demonstrate that by changing the relative delay between the two-color laser fields, we can control the duration of the attosecond bursts from 450 as to 1.2 fs. (C) 2017 Optical Society of America

The evolution of the electronic band structure of the simple ferromagnets Fe, Co, and Ni during their well-known ferromagnetic-paramagnetic phase transition has been under debate for decades, with no clear and even contradicting experimental observations so far. Using time- and spin-resolved photoelectron spectroscopy, we can make a movie on how the electronic properties change in real time after excitation with an ultrashort laser pulse. This allows us to monitor large transient changes in the spin-resolved electronic band structure of cobalt for the first time. We show that the loss of magnetization is not only found around the Fermi level, where the states are affected by the laser excitation, but also reaches much deeper into the electronic bands. We find that the ferromagnetic-paramagnetic phase transition cannot be explained by a loss of the exchange splitting of the spin-polarized bands but instead shows rapid band mirroring after the excitation, which is a clear signature of extremely efficient ultrafast magnon generation. Our result helps to understand band structure formation in these seemingly simple ferromagnetic systems and gives first clear evidence of the transient processes relevant to femtosecond demagnetization.

Attosecond spectroscopic techniques have made it possible to measure differences in transport times for photoelectrons from localized core levels and delocalized valence bands in solids. We report the application of attosecond pulse trains to directly and unambiguously measure the difference in lifetimes between photoelectrons born into free electron-like states and those excited into unoccupied excited states in the band structure of nickel (111). An enormous increase in lifetime of 212 ± 30 attoseconds occurs when the final state coincides with a short-lived excited state. Moreover, a strong dependence of this lifetime on emission angle is directly related to the final-state band dispersion as a function of electron transverse momentum. This finding underscores the importance of the material band structure in determining photoelectron lifetimes and corresponding electron escape depths.

Using laser-dressed photoelectron spectroscopy from solids, we completely characterized the circularly polarized harmonics and reconstructed the complex 3D waveform of the circularly polarized attosecond pulse train.

Using laser-dressed photoelectron spectroscopy from solids, we fully characterize circularly polarized harmonics for the first time to reconstruct the complex 3D waveform of a circularly polarized attosecond pulse train.

We present the first circularly polarized harmonics in the soft X-ray region, enabling the first X-ray magnetic circular dichroism measurements and spin dynamics in rare earth elements such as Gd on a tabletop.

We use attosecond pulse trains to directly measure photoelectron lifetimes in Ni(111) and Cu(111). We observe a strong influence of material band structure on the measured lifetimes, which reveal attosecond timescale electron screening and scattering.

We use attosecond pulse trains to directly measure photoelectron lifetimes in Ni(111) and Cu(111). We observe a strong influence of material band structure on the measured lifetimes, which reveal attosecond timescale electron screening and scattering.

Using laser-dressed photoelectron spectroscopy from solids, we completely characterized the circularly polarized harmonics and reconstructed the complex 3D waveform of the circularly polarized attosecond pulse train.